skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Si-centered capped trigonal prism ordering in liquid Pd 82Si 18 alloy study by first-principles calculations

Abstract

First-principles molecular dynamic (MD) simulation and X-ray diffraction were employed to study the local structures of Pd–Si liquid at the eutectic composition (Pd 82Si 18). Here, a strong repulsion is found between Si atoms, and Si atoms prefer to be evenly distributed in the liquid. The dominate local structures around Si atoms are found to be with of a trigonal prism capped by three half-octahedra and an archimedean anti-prism. The populations of these clusters increase significantly upon cooling, and may play an important role in the formation of Pd 82Si 18 alloy glass.

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [1];  [1];  [3];  [4];  [5];  [3];  [1];  [2];  [6];  [3];  [3];  [1]
  1. Fudan Univ., Shanghai (China). Shanghai Ultra-Precision Optical Manufacturing Engineering Center, Dept. of Optical Science and Engineering
  2. (United States). Dept. of Physics and Astronomy
  3. Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy
  4. National Taiwan Science Education Center, Taipei (Taiwan). Experimentation Division
  5. (Taiwan)
  6. (MoE), Shanghai (China)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation of China; Ministry of Science and Technology of Taiwan
OSTI Identifier:
1355403
Report Number(s):
IS-J-9248
Journal ID: ISSN 2046-2069; RSCACL
Grant/Contract Number:
AC02-07CH11358; AC02-06CH11357; MOST-104-2112-M-492-001; 11374055; 61427815
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 7; Journal Issue: 29; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; First-principles molecular dynamics; x-ray diffraction; Local structure; PdSi alloy

Citation Formats

Dong, F., Yue, G. Q., Ames Lab. and Iowa State Univ., Ames, IA, Guo, Y. R., Qiao, C., Wang, Z. Y., Zheng, Y. X., Zhang, R. J., Sun, Y., Su, W. S., National Taipei Univ. of Technology, Taipei, Kramer, M. J., Wang, S. Y., Ames Lab. and Iowa State Univ., Ames, IA, Key Lab. for Information Science of Electromagnetic Waves, Wang, C. Z., Ho, K. M., and Chen, L. Y. Si-centered capped trigonal prism ordering in liquid Pd82Si18 alloy study by first-principles calculations. United States: N. p., 2017. Web. doi:10.1039/c6ra28232f.
Dong, F., Yue, G. Q., Ames Lab. and Iowa State Univ., Ames, IA, Guo, Y. R., Qiao, C., Wang, Z. Y., Zheng, Y. X., Zhang, R. J., Sun, Y., Su, W. S., National Taipei Univ. of Technology, Taipei, Kramer, M. J., Wang, S. Y., Ames Lab. and Iowa State Univ., Ames, IA, Key Lab. for Information Science of Electromagnetic Waves, Wang, C. Z., Ho, K. M., & Chen, L. Y. Si-centered capped trigonal prism ordering in liquid Pd82Si18 alloy study by first-principles calculations. United States. doi:10.1039/c6ra28232f.
Dong, F., Yue, G. Q., Ames Lab. and Iowa State Univ., Ames, IA, Guo, Y. R., Qiao, C., Wang, Z. Y., Zheng, Y. X., Zhang, R. J., Sun, Y., Su, W. S., National Taipei Univ. of Technology, Taipei, Kramer, M. J., Wang, S. Y., Ames Lab. and Iowa State Univ., Ames, IA, Key Lab. for Information Science of Electromagnetic Waves, Wang, C. Z., Ho, K. M., and Chen, L. Y. Fri . "Si-centered capped trigonal prism ordering in liquid Pd82Si18 alloy study by first-principles calculations". United States. doi:10.1039/c6ra28232f. https://www.osti.gov/servlets/purl/1355403.
@article{osti_1355403,
title = {Si-centered capped trigonal prism ordering in liquid Pd82Si18 alloy study by first-principles calculations},
author = {Dong, F. and Yue, G. Q. and Ames Lab. and Iowa State Univ., Ames, IA and Guo, Y. R. and Qiao, C. and Wang, Z. Y. and Zheng, Y. X. and Zhang, R. J. and Sun, Y. and Su, W. S. and National Taipei Univ. of Technology, Taipei and Kramer, M. J. and Wang, S. Y. and Ames Lab. and Iowa State Univ., Ames, IA and Key Lab. for Information Science of Electromagnetic Waves and Wang, C. Z. and Ho, K. M. and Chen, L. Y.},
abstractNote = {First-principles molecular dynamic (MD) simulation and X-ray diffraction were employed to study the local structures of Pd–Si liquid at the eutectic composition (Pd82Si18). Here, a strong repulsion is found between Si atoms, and Si atoms prefer to be evenly distributed in the liquid. The dominate local structures around Si atoms are found to be with of a trigonal prism capped by three half-octahedra and an archimedean anti-prism. The populations of these clusters increase significantly upon cooling, and may play an important role in the formation of Pd82Si18 alloy glass.},
doi = {10.1039/c6ra28232f},
journal = {RSC Advances},
number = 29,
volume = 7,
place = {United States},
year = {Fri Mar 24 00:00:00 EDT 2017},
month = {Fri Mar 24 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2works
Citation information provided by
Web of Science

Save / Share:
  • The medium range order (MRO) and its relation to the structural decomposition on annealing in Pd-Si amorphous alloys have been studied by high resolution electron microscopy, nano-beam electron diffraction and nano-beam elemental analysis. Amorphous Pd[sub 82]Si[sub 18] thin film specimens were prepared by Ar-beam sputtering. The f.c.c. MRO domains were observed in the as-sputtered films. On annealing, observation frequency and the size of the MRO domains were observed in the as-sputtered films. On annealing, observation frequency and the size of the MRO domains increased. The f.c.c. MRO domains grew to nano-precipitates of [alpha]-Pd after annealing at 573 K. At thismore » stage, the second halo diffraction ring tends to split into two in the selected area electron diffraction patterns. The Si atoms are thought to occupy octahedral interstices in the small precipitates and diffuse out to the matrix with increasing the precipitate sizes. The Si composition in the nano-precipitates decreases in the course of growth. It is concluded that the atomic free volume is annihilated by the atomic rearrangement in the formation and development of MRO domains, and that chemical ordering is developed in the surrounding matrix by the local compositional change. The structural relaxation must be corresponding to these local atomic structural changes.« less
  • First-principles calculations based on density-functional theory in the pseudopotential approach have been performed for the energetics and crystal structure of Y{sub 2}Si{sub 3}O{sub 3}N{sub 4} with the melilite-type structure. The calculations show the following ordering of the O/N atoms in the crystal: N atoms fully occupy the bridging site (2c) and O atoms fully occupy the terminal site (4e) WITH 2 O and 6 N atoms at the bridging 8f site. These conclusions are in good agreement with the experimental results obtained with neutron diffraction. In addition, the calculations show that there is a preferential distribution of the O andmore » N atoms at the 8f site, resulting in two different local coordinations of Y, as compared to only a single averaged crystallographic Y site. All the nitrogen ions exhibit similar electronic structure, in contrast to the oxygen ions. However, there are slightly more electrons (about 0.1 electrons per ion) for nitrogen at the 2c site than those at the 8f site, while the silicon atoms have almost the same charge distribution.« less
  • In the present work, we have used density functional theory (DFT) and DFT+U to investigate the crystal structure and phase stability of four model compounds in the Ln 2O 3-UO 2-UO 3 ternary oxide system: La2UO 6, Ce 2UO 6, LaUO 4, CeUO 4, due to the highly-correlated nature of the f-electrons in uranium. We have considered both hypothetical ordered compounds and compounds in which the cations randomly occupy atomic sites in a fluorite-like lattice. We determined that ordered compounds are stable and are energetically favored compared to disordered configurations, though the ordering tendencies are weak. To model and analyzemore » the structures of these complex oxides, we have used supercells based on a layered atomic model. In the layer model, the supercell is composed of alternating planes of anions and cations. We have considered two different ordering motifs for the cations, namely single species (isoatomic) cation layers versus mixed species cation layers. Energy differences between various ordered cationic arrangements were found to be small. This may have implications regarding radiation stability, since cationic arrangements should be able to change under irradiation with little cost in energy.« less
  • First-principles molecular dynamics simulations of the Pd(001)/3C–SiC(001) nano-layered structure were carried out at different temperatures ranging from 300 to 2100 K. Various PdSi (Pnma, Fm3m, P6m2, Pm3m), Pd 2Si (P6⁻2m, P6 3/mmc, P3m1, P3⁻1m) and Pd 3Si (Pnma, P6 322, Pm3m, I4/mmm) structures under pressure were studied to identify the structure of the Pd/Si and Pd/C interfaces in the Pd/SiC systems at high temperatures. It was found that a large atomic mixing at the Pd/Si interface occurred at 1500–1800 K, whereas the Pd/C interface remained sharp even at the highest temperature of 2100 K. At the Pd/C interface, voids andmore » a graphite-like clustering were detected. Palladium and silicon atoms interact at the Pd/Si interface to mostly form C22-Pd 2Si and D0 11-Pd 3Si fragments, in agreement with experiment.« less